Engineering of Amorphous Structures and Sulfur Defects into Ultrathin FeS Nanosheets to Achieve Superior...

Integration of amorphous structures and anion defects into ultrathin 2D materials has been identified as an effective strategy for boosting the electrocatalytic performance. However, the in-depth understanding of the relationship among the amorphous structure, vacancy defect, and catalytic activity is still obscure. Herein, a facile strategy was proposed to prepare ultrathin and amorphous Mo-FeS nanosheets (NSs) with abundant sulfur defects. Benefited from the ultrathin, amorphous nanostructure, and synergy effect of Mo-doping and sulfur defect, the Mo-FeS NSs manifested excellent electrocatalytic activity toward oxygen evolution reaction (OER) in alkaline medium, as shown by an ultralow overpotential of 210 mV at 10 mA cm^-2, a Tafel slope of 50 mV dec^-1, and retaining such good catalytic stability over 30 h. The efficient catalytic performance for Mo-FeS NSs is superior to the commercial IrO₂ and most reported top-performing electrocatalysts. Density functional theory calculations revealed that the accelerated electron/mass transfer over the oxygen-containing intermediates can be attributed to the amorphous structure and sulfur-rich defects caused by structural reconfiguration. Furthermore, the S vacancies could enhance the activity of its neighboring Fe-active sites, which was also beneficial to their OER kinetics. This work integrated both amorphous structures and sulfur vacancies into ultrathin 2D NSs and further systematically evaluated the OER performance, providing new insights for the design of amorphous-layered electrocatalysts.